Singlet oxygen(^(1)O_(2))is recognized as one of the most effective and selective oxygen agents.However,the explorative study of photocatalysts(PCs)for effective ^(1)O_(2)-based photocatalytic oxidation remains challe...Singlet oxygen(^(1)O_(2))is recognized as one of the most effective and selective oxygen agents.However,the explorative study of photocatalysts(PCs)for effective ^(1)O_(2)-based photocatalytic oxidation remains challenging and critical.In this study,a novel donor-acceptor metal-organic framework(D-A MOF)has been developed by engineering the D-A system,which was then evaluated as a photocatalyst for ^(1)O_(2)-based oxidation.By regulating the donor component of the D-A systematic framework,the MOF(B1)exhibits delayed fluorescence(DF)behavior with a reduced singlet-triplet gap.Given the significantly improved electron transfer behavior in combination with an efficient energy transfer process,the optimal B1 demonstrates remarkable activity toward ^(1)O_(2)generation under suitable photoexcitation conditions.Therefore,it can be utilized for the photocatalytic oxidation of 1,5-dioxynaphthalene(1,5-DHN)to Juglone,achieving the highest yield(conversion>99%at 25℃ in 30 min)and selectivity among all previously reported MOF photocatalysts.展开更多
BaFe_(12)O_(19)(BaM)thin films with thicknesses ranging from 15 nm–200 nm were deposited on Al_(2)O_(3)(0001)substrates by pulsed laser deposition(PLD).X-ray diffraction patterns show that a buffer layer with a thick...BaFe_(12)O_(19)(BaM)thin films with thicknesses ranging from 15 nm–200 nm were deposited on Al_(2)O_(3)(0001)substrates by pulsed laser deposition(PLD).X-ray diffraction patterns show that a buffer layer with a thickness of nearly 60 nm forms on the substrate,and then a c-axis perpendicularly oriented Ba M thin film grows on the buffer layer.Atomic force microscopy results indicate that the Ba M thin film exhibits a spiral island growth mode on the buffer layer.Magnetic hysteresis loop results confirm that the buffer layer exhibits no significant magnetic anisotropy,while the Ba M thin film exhibits perpendicular magnetic anisotropy.The out-of-plane coercivity decreases with increasing Ba M thin-film thickness due to the combined effect of grain size growth and lattice strain relaxation.The 200 nm thick film exhibits optimum magnetic properties with M_(s)=319 emu/cm^(3) and H_(c)=1546 Oe.展开更多
When stacking two-dimensional(2D)materials with a lattice mismatch and/or a small twist,moirésuperlattice emerges with fascinating electronic and optical properties.The fabrication of such stacked 2D materials us...When stacking two-dimensional(2D)materials with a lattice mismatch and/or a small twist,moirésuperlattice emerges with fascinating electronic and optical properties.The fabrication of such stacked 2D materials usually requires multiple transfer and stack processes,assisted by a certain transfer medium which needs to be removed afterwards,and it is very challenging to maintain pristine and clean surfaces/interfaces for these stacked structures.In this work,we report a facile direct bonding method for fabrication of twisted MoS_(2) bilayers with ultra-clean surfaces/interfaces.Novel interlayer interactions are revealed in the as-fabricated high-quality samples,leading to twist-angle related dispersion behavior of various Raman modes,such as layer breathing modes,shear modes and E_(2g)modes,as well as indirect bandgap excitons.Field-effect transistors(FETs)of twisted MoS_(2) bilayers also exhibit angle-dependent performance,which could be attributed to the band structure evolution.This facile method holds significance for the future integration of pre-designed multilayer 2D materials and paves a way to explore underlying physical mechanisms and potential applications.展开更多
The electrocatalytic reduction of carbon dioxide(CO_(2)RR)to valuable products presents a promising solution for addressing global warming and enhancing renewable energy storage.Herein,we construct a novel Ni_(3)ZnC_(...The electrocatalytic reduction of carbon dioxide(CO_(2)RR)to valuable products presents a promising solution for addressing global warming and enhancing renewable energy storage.Herein,we construct a novel Ni_(3)ZnC_(0.7)/Ni heterostructure electrocatalyst,using an electrospinning strategy to prepare metal particles uniformly loaded on nitrogen-doped carbon nanofibers(CNFs).The incorporation of zinc(Zn)into nickel(Ni)catalysts optimizes the adsorption of CO_(2)intermediates,balancing the strong binding affinity of Ni with the comparatively weaker affinity of Zn,which mitigates over-activation.The electron transfer within the Ni_(3)ZnC_(0.7)/Ni@CNFs system facilitates rapid electron transfer to CO_(2),resulting in great performance with a faradaic efficiency for CO(FECO)of nearly 90%at−0.86 V versus the reversible hydrogen electrode(RHE)and a current density of 17.51 mA cm^(−2)at−1.16 V versus RHE in an H-cell.Furthermore,the catalyst exhibits remarkable stability,maintaining its crystal structure and morphology after 50 h of electrolysis.Moreover,the Ni_(3)ZnC_(0.7)/Ni@CNFs is used in the membrane electrode assembly reactor(MEA),which can achieve a FECO of 91.7%at a cell voltage of−3 V and a current density of 200 mA cm−2 at−3.9 V,demonstrating its potential for practical applications in CO_(2)reduction.展开更多
Aqueous zinc metal batteries(AZMBs)are promising candidates for next-generation energy storage,but their commercialization is hindered by zinc anode challenges,notably parasitic reactions and dendrite growth.Herein,we...Aqueous zinc metal batteries(AZMBs)are promising candidates for next-generation energy storage,but their commercialization is hindered by zinc anode challenges,notably parasitic reactions and dendrite growth.Herein,we present a biodegradable biomass-derived protective layer,primarily composed of curcumin,as a zincophilic interface for AZMBs.The curcumin-based layer,fabricated via a homogeneous solution process,exhibits strong adhesion,uniform coverage,and robust mechanical integrity.Rich polar functional groups in curcumin facilitate homogeneous Zn~(2+)flux and suppress side reactions.The curcumin-based layer shows a favorable affinity for zinc trifluoromethanesulfonate(Zn(OTf)_(2))electrolyte,which is the representative of organic zinc salts,enabling optimal thickness for both protection and ion transport.The protected Zn anodes demonstrate an extended lifespan of 2500 h in symmetrical cells and a high Coulombic efficiency of 99.15%.Furthermore,Zn(OTf)_(2)-based system typically exhibits poor stability at high current densities.Fortunately,the lifespan of symmetrical cells was extended by 40-fold at the high current density.When paired with an Na V_(3)O_(8)·1.5H_(2)O(NVO)cathode,the system achieves 86.5%capacity retention after 3000 cycles at a large specific current density of 10 A g^(-1).These results underscore the efficacy of the curcumin-based protective layer in enhancing the reversibility and stability of metal electrodes,specifically relieving the instability of Zn(OTf)_(2)-based systems at high current densities,advancing its commercial viability.展开更多
The thermodynamic properties of the ε phase of solid oxygen are studied by using the analytic mean field approach （AMFP）. Analytic expressions for the Helmholtz free energy, internal energy and equation of state of...The thermodynamic properties of the ε phase of solid oxygen are studied by using the analytic mean field approach （AMFP）. Analytic expressions for the Helmholtz free energy, internal energy and equation of state of solid oxygen have been derived based on the multi-exponential potential. The formulism for the case of double-exponential （DE） model is applied to the ε phase of solid oxygen. Its four potential parameters are determined through fitting the experimental compression data of the ε phase of solid oxygen. Numerical results of the pressure dependence of the volume calculated by using the AMFP are in good agreement with the original experimental data. This suggests that the AMFP is a useful approach to study the thermodynamic properties of the ε phase of solid oxygen. Furthermore, we predict the variation of the volume, lattice parameters and intermolecular distances with pressure, and some thermodynamic quantities versus volume, at several higher temperatures.展开更多
It is important to know whether the laws or phenomena in statistical physics for natural systems with non-adaptive agents still hold for social human systems with adaptive agents, because this implies whether it is po...It is important to know whether the laws or phenomena in statistical physics for natural systems with non-adaptive agents still hold for social human systems with adaptive agents, because this implies whether it is possible to study or understand social human systems by using statistical physics originating from natural systems. For this purpose, we review the role of human adaptability in four kinds of specific human behaviors, namely, normal behavior, herd behavior, contrarian behavior, and hedge behavior. The approach is based on controlled experiments in the framework of market-directed resource-allocation games. The role of the controlled experiments could be at least two-fold： adopting the real human decision-making process so that the system under consideration could reflect the performance of genuine human beings; making it possible to obtain macroscopic physical properties of a human system by tuning a particular factor of the system, thus directly revealing cause and effect. As a result, both computer simulations and theoretical analyses help to show a few counterparts of some laws or phenomena in statistical physics for social human systems： two-phase phenomena or phase transitions, entropy-related phenomena, and a non-equilibrium steady state. This review highlights the role of human adaptability in these counterparts, and makes it possible to study or understand some particular social human systems by means of statistical physics coming from natural systems.展开更多
Since the first demonstrations of nuclear magnetic resonance (NMR) in condensed matter in 1946, the field of NMR has yielded a continuous flow of conceptual advances and methodological innovations that continues today...Since the first demonstrations of nuclear magnetic resonance (NMR) in condensed matter in 1946, the field of NMR has yielded a continuous flow of conceptual advances and methodological innovations that continues today. Much progress has been made in the utilization of solid-state NMR to illuminate molecular structure and dynamics in systems not controllable by any other way. NMR deals with time-dependent perturbations of nuclear spin systems and solving the time-dependent Schrodinger equation is a central problem in quantum physics in general and solid-state NMR in particular. This theoretical perspective outlines the methods used to treat theoretical problems in solid-state NMR as well as the recent theoretical development of spin dynamics in NMR and physics. The purpose of this review is to unravel the versatility of theories in solid-state NMR and to present the recent theoretical developments of spin dynamics.展开更多
We study theoretically the electron transport properties in achiral carbon nanotubes under the influence of an external electric field E(t) using Boltzmann’s transport equation to derive the current-density. A negati...We study theoretically the electron transport properties in achiral carbon nanotubes under the influence of an external electric field E(t) using Boltzmann’s transport equation to derive the current-density. A negative differential conductivity (NDC) is predicted in quasi-static approximation i.e., ωτ 0 is equal to the amplitude of the AC electric field E1. The peak of the NDC intensity occurs at very weaker fields than that of superlattice under the same conditions. The peak intensity decreases and shifts to right with the increase in the amplitude of the ac field. This mechanism suppresses the domain formation and therefore could be used in terahertz frequency generation.展开更多
The growth of computing power in data centers(DCs)leads to an increase in energy consumption and noise pollution of air cooling systems.Chip-level cooling with high-efficiency coolant is one of the promising methods t...The growth of computing power in data centers(DCs)leads to an increase in energy consumption and noise pollution of air cooling systems.Chip-level cooling with high-efficiency coolant is one of the promising methods to address the cooling challenge for high-power devices in DCs.Hybrid nanofluid(HNF)has the advantages of high thermal conductivity and good rheological properties.This study summarizes the numerical investigations of HNFs in mini/micro heat sinks,including the numerical methods,hydrothermal characteristics,and enhanced heat transfer technologies.The innovations of this paper include:(1)the characteristics,applicable conditions,and scenarios of each theoretical method and numerical method are clarified;(2)the molecular dynamics(MD)simulation can reveal the synergy effect,micro motion,and agglomeration morphology of different nanoparticles.Machine learning(ML)presents a feasiblemethod for parameter prediction,which provides the opportunity for the intelligent regulation of the thermal performance of HNFs;(3)the HNFs flowboiling and the synergy of passive and active technologies may further improve the overall efficiency of liquid cooling systems in DCs.This review provides valuable insights and references for exploring the multi-phase flow and heat transport mechanisms of HNFs,and promoting the practical application of HNFs in chip-level liquid cooling in DCs.展开更多
The stability of perovskite solar cells(PSCs)is adversely affected by nonradiative recombination resulting from buried interface defects.Herein,we synthesize a polyionic liquid,poly(p-vinylbenzyl trimethylam-monium he...The stability of perovskite solar cells(PSCs)is adversely affected by nonradiative recombination resulting from buried interface defects.Herein,we synthesize a polyionic liquid,poly(p-vinylbenzyl trimethylam-monium hexafluorophosphate)(PTA),and introduce it into the buried interface of PSCs.The quaternary ammonium cation(N(-CH_(3))^(3+))in PTA can fill the vacancies of organic cations within the perovskite structure and reduce shallow energy level defects.Additionally,the hexafluorophosphate(PF6−)in PTA forms a Lewis acid-base interaction with Pb^(2+)in the perovskite layer,effectively passivating deep en-ergy level defects.Furthermore,hydrogen bonding can be established between organic cations and the PF6−anion,preventing the formation of shallow energy level defects.Through this synergistic mecha-nism,the deep and shallow energy level defects are effectively mitigated,resulting in improved device performance.As a result,the resulting treated inverted PSC exhibits an impressive power conversion ef-ficiency(PCE)of 24.72%.Notably,the PTA-treated PSCs exhibit remarkable stability,with 88.5%of the original PCE retained after undergoing heat aging at 85℃ for 1078 h,and 89.1%of the initial PCE main-tained following continuous exposure to light for 1100 h at the maximum power point.Synergistically suppressing multiple defects at the buried interface through the use of polyionic liquids is a promising way to improve the commercial viability of PSCs.展开更多
Fueled by the increasing imperative for sustainable energy solutions and the burgeoning emphasis on health awareness,self-powered techniques have undergone notable strides in advancement.Triboelectric nanogenerators(T...Fueled by the increasing imperative for sustainable energy solutions and the burgeoning emphasis on health awareness,self-powered techniques have undergone notable strides in advancement.Triboelectric nanogenerators(TENGs)stand out as a prominent device capitalizing on the principles of triboelectrification and electrostatic induction to generate electricity or electrical signals.In efforts to augment the electrical output performance of TENGs and broaden their range of applications,researchers have endeavored to refine materials,surface morphology,and structural design.Among them,physical morphological modifications play a pivotal role in enhancing the electrical properties of TENGs by increasing the contact surface area,which can be achieved by building micro-/nano-structures on the surface or inside the friction material.In this review,we summarize the common morphologies of TENGs,categorize the morphologies into surface and internal structures,and elucidate their roles in enhancing the electric output performance of devices.Moreover,we systematically classify the methodologies employed for morphological preparation into physical and chemical approaches,thereby furnishing a comprehensive survey of the diverse techniques.Subsequently,typical applications of TENGs with special morphology divided by energy harvesting and self-powered sensors are presented.Finally,an overview of the challenges and future trajectories pertinent to TENGs is conducted.Through this endeavor,the aim of this article is to catalyze the evolution of further strategies for enhancing performance of TENGs.展开更多
High-resolution transmission electron microscopy(HRTEM)promises rapid atomic-scale dynamic structure imaging.Yet,the precision limitations of aberration parameters and the challenge of eliminating aberrations in Cs-co...High-resolution transmission electron microscopy(HRTEM)promises rapid atomic-scale dynamic structure imaging.Yet,the precision limitations of aberration parameters and the challenge of eliminating aberrations in Cs-corrected transmission electron microscopy constrain resolution.A machine learning algorithm is developed to determine the aberration parameters with higher precision from small,lattice-periodic crystal images.The proposed algorithm is then validated with simulated HRTEM images of graphene and applied to the experimental images of a molybdenum disulfide(MoS_(2))monolayer with 25 variables(14 aberrations)resolved in wide ranges.Using these measured parameters,the phases of the exit-wave functions are reconstructed for each image in a focal series of MoS_(2)monolayers.The images were acquired due to the unexpected movement of the specimen holder.Four-dimensional data extraction reveals time-varying atomic structures and ripple.In particular,the atomic evolution of the sulfur-vacancy point and line defects,as well as the edge structure near the amorphous,is visualized as the resolution has been improved from about 1.75?to 0.9 A.This method can help salvage important transmission electron microscope images and is beneficial for the images obtained from electron microscopes with average stability.展开更多
The sodium-ion battery(SIB)cathode material,Na_(4)Fe_(3)(PO_(4))_(2)(P_(2)O_(7))(NFPP),has become a focal material in both academia and industry due to its low cost,long lifespan,and high safety.In the recent three ye...The sodium-ion battery(SIB)cathode material,Na_(4)Fe_(3)(PO_(4))_(2)(P_(2)O_(7))(NFPP),has become a focal material in both academia and industry due to its low cost,long lifespan,and high safety.In the recent three years,substantial efforts have been devoted to promoting the practical applications of NFPP by optimizing its electrochemical performance and disclosing the reaction mechanisms.Various modification strategies and their effect mechanisms have been explored,and the performance evaluation of NFPP has progressively advanced from laboratory-scale coin cells to practical pouch cell configurations.Nevertheless,there remains a lack of systematic reviews comprehensively assessing the developmental status and application readiness of NFPP.This review critically examines NFPP's fundamental structural characteristics and proposes four key development issues.Then,the latest research advances are introduced with explicit differentiation of design strategies and their mechanistic impacts.Notably,we provide a dedicated discussion on NFPP's current pouch cell performance metrics,while highlighting two critical yet underexplored research directions(enhancing air stability and improving tap density)for commercial viability.展开更多
An experimental investigation of the dynamics of the interface between two low-viscosity fluids with high density contrast oscillating in a fixed vertical slotted channel has been conducted.It has been found that as t...An experimental investigation of the dynamics of the interface between two low-viscosity fluids with high density contrast oscillating in a fixed vertical slotted channel has been conducted.It has been found that as the amplitude of the liquid column oscillations increases,parametric oscillations of the interface are excited in the form of a standing wave located in the channel plane.In particular,depending on the interfacial tension,the standing waves have a frequency equal to that of liquid piston oscillations(harmonic response),or half of the frequency of oscillations of the liquid column in the channel(subharmonic response).The detected type of instability has a gravitational-capillary nature and is analogous to Faraday waves.The analysis of the overcritical dynamics of wave oscillations indicates that interfacial tension plays a crucial role in determining the type of parametric instability.At high interfacial tension,only synchronous(harmonic)wave modes are observed,and the threshold of the wave excitation is determined by the amplitude of piston oscillations of the liquid column.In this case,the oscillation acceleration does not play a role and has a small value in the threshold of the synchronous mode response.In the case of weak surface tension,subharmonic oscillations are observed.The threshold for the development of these oscillations is determined by the dimensionless acceleration of the oscillating liquid column and remains almost constant with variations in the dimensionless frequency of oscillations.At moderate values of interfacial tension(in the region of moderate dimensionless frequencies),a synchronous wave mode emerges in the stability threshold of the oscillating interface.As the dimensionless acceleration is increased further,a subharmonic mode is excited.The growth of subharmonic oscillations occurs against the background of harmonic wave oscillations,with the oscillations of the interface representing a combination of two standing waves.展开更多
LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811)is an attractive material for high-energy-density Li-ion batteries in electric vehicles.However,it suffers from rapid capacity fading.Previous studies have shown that tuning the ...LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811)is an attractive material for high-energy-density Li-ion batteries in electric vehicles.However,it suffers from rapid capacity fading.Previous studies have shown that tuning the positive electrode material via atomic layer deposition(ALD)can enhance the electrochemical performance of the material.In this article,we introduce a novel coating method using gaseous precursors in an ALD reactor,where an AlO_(x)layer is deposited directly on the surface of the NMC811 precursor,followed by lithiation.The AlO_(x)coating is applied to the NMC811 powder substrate by exposing it to gas-phase precursors,using a conventional ALD and simplified ALD(chemical vapor deposition-like)method.It is observed that the novel methods lead to the incorporation of Al as a dopant within the bulk of NMC811,rather than forming a conformal AlO_(x)coating,after the final lithiation step.The optimized procedures result in positive electrode materials with higher capacity and enhanced cycling stability in both half-cell and full-cell configurations.Doping or coating was shown to mitigate transition metal dissolution,reduce side reactions between the active material and electrolyte,and improve structural stability.展开更多
The gravitational memory effect manifests gravitational nonlinearity,degenerate vacua,and asymptotic symmetries;its detection is considered challenging.We propose using a space-borne interferometer to detect memory si...The gravitational memory effect manifests gravitational nonlinearity,degenerate vacua,and asymptotic symmetries;its detection is considered challenging.We propose using a space-borne interferometer to detect memory signals from stellar-mass binary black holes(BBHs),typically targeted by ground-based detectors.We use DECIGO detector as an example.Over 5 years,DECIGO is estimated to detect approximately 2,036 memory signals(SNRs>3)from stellar-mass BBHs.Simulations used frequency-domain memory waveforms for direct SNR estimation.Predictions utilized a GWTC-3 constrained BBH population model(Power law+Peak mass,DEFAULT spin,Madau-Dickinson merger rate).The analysis used conservative lower merger rate limits and considered orbital eccentricity.The high detection rate stems from strong memory signals within DECIGO’s bandwidth and the abundance of stellar-mass BBHs.This substantial and conservative detection count enables statistical use of the memory effect for fundamental physics and astrophysics.DECIGO exemplifies that space interferometers may better detect memory signals from smaller mass binaries than their typical targets.Detectors in lower frequency bands are expected to find strong memory signals from∼10^(4)M⊙binaries.展开更多
This paper investigates the influence of filling fraction on the segregation patterns of binary granular mixtures in a vertically vibrating drum through experiments and simulations.Glass and stainless steel spherical ...This paper investigates the influence of filling fraction on the segregation patterns of binary granular mixtures in a vertically vibrating drum through experiments and simulations.Glass and stainless steel spherical grains,which differ in mass density,are used to give rise to density-driven segregation.The results reveal four segregation patterns,including Brazil nut effect segregation,counterclockwise two-eye-like segregation,dumpling-like segregation and clockwise twoeye-like segregation.The theoretical analysis demonstrates that grains predominantly exhibit counterclockwise convection at low filling fractions,while clockwise convection dominates at high filling fractions.Competition between buoyancy and convection forces determines the final stable segregation pattern.These findings provide valuable insights into controlling segregation in granular systems,which is crucial for optimizing industrial processes in fields such as pharmaceuticals and chemical engineering.展开更多
Iron-chromium flow batteries(ICRFBs)have emerged as an ideal large-scale energy storage device with broad application prospects in recent years.Enhancement of the Cr^(3+)/Cr^(2+)redox reaction activity and inhibition ...Iron-chromium flow batteries(ICRFBs)have emerged as an ideal large-scale energy storage device with broad application prospects in recent years.Enhancement of the Cr^(3+)/Cr^(2+)redox reaction activity and inhibition of the hydrogen evolution side reaction(HER)are essential for the development of ICRFBs and require a novel catalyst design.However,elucidating the underlying mechanisms for modulating catalyst behaviors remains an unresolved challenge.Here,we show a novel precisely controlled preparation of a novel thermal-treated carbon cloth electrode with a uniform deposit of low-cost indium catalyst particles.The density functional theory analysis reveals the In catalyst has a significant adsorption effect on the reactants and improves the redox reaction activity of Cr^(3+)/Cr^(2+).Moreover,H+is more easily absorbed on the surface of the catalyst with a high migration energy barrier,thereby inhibiting the occurrence of HER.The assembled ICRFBs have an average energy efficiency of 83.91%at 140 mA cm^(-2),and this method minimizes the electrodeposition process and cleans the last obstacle for industry long cycle operation requirements.The ICRFBs exhibit exceptional long-term stability with an energy efficiency decay rate of 0.011%per cycle at 1000 cycles,the lowest ICRFBs reported so far.Therefore,this study provides a promising strategy for developing ICRFBs with low costs and long cycle life.展开更多
The effects of synthesis conditions,especially the heating rate,on the reaction kinetics of Ni-rich cathodes were systematically studied.The growth rate of Ni-rich oxide increases continuously as the heating rate incr...The effects of synthesis conditions,especially the heating rate,on the reaction kinetics of Ni-rich cathodes were systematically studied.The growth rate of Ni-rich oxide increases continuously as the heating rate increases.Ab initio molecular dynamics simulations demonstrate that a high heating rate induces anabatic oscillations,indicating a decrease in thermodynamic stability and a tendency for the crystal surface to undergo reconstruction.The presence of an intermediate phase at the grain boundary amplifies atomic migration-induced interface fusion and consequently augments crystal growth kinetics.However,the excessively high heating rate aggravates the Li+/Ni2+mixing in the Ni-rich cathode.The single-crystal Ni-rich cathode exhibits enhanced structural/thermal stability but a decreased specific capacity and rate performance compared with its polycrystalline counterpart.展开更多
基金supported by the National Key R&D Program of China(2022YFA1503301)the National Natural Science Foundation of China(NSFC)(22375104,22035003,22201143,22371134)+1 种基金the China Postdoctoral Science Foundation(2022M711699)the Haihe Laboratory of Sustainable Chemical Transformations(YYJC202101)。
文摘Singlet oxygen(^(1)O_(2))is recognized as one of the most effective and selective oxygen agents.However,the explorative study of photocatalysts(PCs)for effective ^(1)O_(2)-based photocatalytic oxidation remains challenging and critical.In this study,a novel donor-acceptor metal-organic framework(D-A MOF)has been developed by engineering the D-A system,which was then evaluated as a photocatalyst for ^(1)O_(2)-based oxidation.By regulating the donor component of the D-A systematic framework,the MOF(B1)exhibits delayed fluorescence(DF)behavior with a reduced singlet-triplet gap.Given the significantly improved electron transfer behavior in combination with an efficient energy transfer process,the optimal B1 demonstrates remarkable activity toward ^(1)O_(2)generation under suitable photoexcitation conditions.Therefore,it can be utilized for the photocatalytic oxidation of 1,5-dioxynaphthalene(1,5-DHN)to Juglone,achieving the highest yield(conversion>99%at 25℃ in 30 min)and selectivity among all previously reported MOF photocatalysts.
文摘BaFe_(12)O_(19)(BaM)thin films with thicknesses ranging from 15 nm–200 nm were deposited on Al_(2)O_(3)(0001)substrates by pulsed laser deposition(PLD).X-ray diffraction patterns show that a buffer layer with a thickness of nearly 60 nm forms on the substrate,and then a c-axis perpendicularly oriented Ba M thin film grows on the buffer layer.Atomic force microscopy results indicate that the Ba M thin film exhibits a spiral island growth mode on the buffer layer.Magnetic hysteresis loop results confirm that the buffer layer exhibits no significant magnetic anisotropy,while the Ba M thin film exhibits perpendicular magnetic anisotropy.The out-of-plane coercivity decreases with increasing Ba M thin-film thickness due to the combined effect of grain size growth and lattice strain relaxation.The 200 nm thick film exhibits optimum magnetic properties with M_(s)=319 emu/cm^(3) and H_(c)=1546 Oe.
基金supported by Guangdong Major Project of Basic and Applied Basic Research(Grant No.2021B0301030002)the National Key Research and Development Program(Grant No.2021YFA1202900)the National Natural Science Foundation of China(Grant Nos.62204166 and 62404145)。
文摘When stacking two-dimensional(2D)materials with a lattice mismatch and/or a small twist,moirésuperlattice emerges with fascinating electronic and optical properties.The fabrication of such stacked 2D materials usually requires multiple transfer and stack processes,assisted by a certain transfer medium which needs to be removed afterwards,and it is very challenging to maintain pristine and clean surfaces/interfaces for these stacked structures.In this work,we report a facile direct bonding method for fabrication of twisted MoS_(2) bilayers with ultra-clean surfaces/interfaces.Novel interlayer interactions are revealed in the as-fabricated high-quality samples,leading to twist-angle related dispersion behavior of various Raman modes,such as layer breathing modes,shear modes and E_(2g)modes,as well as indirect bandgap excitons.Field-effect transistors(FETs)of twisted MoS_(2) bilayers also exhibit angle-dependent performance,which could be attributed to the band structure evolution.This facile method holds significance for the future integration of pre-designed multilayer 2D materials and paves a way to explore underlying physical mechanisms and potential applications.
基金financial support from the Natural Science Foundation of Yancheng(YCBK2024004)the Basic Research Program of Jiangsu(BK20251089)the“Scientific and Technical Innovation Action Plan”Basic Research Field of Shanghai Science and Technology Committee(19JC1410500).
文摘The electrocatalytic reduction of carbon dioxide(CO_(2)RR)to valuable products presents a promising solution for addressing global warming and enhancing renewable energy storage.Herein,we construct a novel Ni_(3)ZnC_(0.7)/Ni heterostructure electrocatalyst,using an electrospinning strategy to prepare metal particles uniformly loaded on nitrogen-doped carbon nanofibers(CNFs).The incorporation of zinc(Zn)into nickel(Ni)catalysts optimizes the adsorption of CO_(2)intermediates,balancing the strong binding affinity of Ni with the comparatively weaker affinity of Zn,which mitigates over-activation.The electron transfer within the Ni_(3)ZnC_(0.7)/Ni@CNFs system facilitates rapid electron transfer to CO_(2),resulting in great performance with a faradaic efficiency for CO(FECO)of nearly 90%at−0.86 V versus the reversible hydrogen electrode(RHE)and a current density of 17.51 mA cm^(−2)at−1.16 V versus RHE in an H-cell.Furthermore,the catalyst exhibits remarkable stability,maintaining its crystal structure and morphology after 50 h of electrolysis.Moreover,the Ni_(3)ZnC_(0.7)/Ni@CNFs is used in the membrane electrode assembly reactor(MEA),which can achieve a FECO of 91.7%at a cell voltage of−3 V and a current density of 200 mA cm−2 at−3.9 V,demonstrating its potential for practical applications in CO_(2)reduction.
基金the financial support from Research Institute for Smart Energy at the Hong Kong Polytechnic University(Grant No.CDB2)the support of the Hong Kong PhD Fellowship Scheme(Grant No.PF21-65328)。
文摘Aqueous zinc metal batteries(AZMBs)are promising candidates for next-generation energy storage,but their commercialization is hindered by zinc anode challenges,notably parasitic reactions and dendrite growth.Herein,we present a biodegradable biomass-derived protective layer,primarily composed of curcumin,as a zincophilic interface for AZMBs.The curcumin-based layer,fabricated via a homogeneous solution process,exhibits strong adhesion,uniform coverage,and robust mechanical integrity.Rich polar functional groups in curcumin facilitate homogeneous Zn~(2+)flux and suppress side reactions.The curcumin-based layer shows a favorable affinity for zinc trifluoromethanesulfonate(Zn(OTf)_(2))electrolyte,which is the representative of organic zinc salts,enabling optimal thickness for both protection and ion transport.The protected Zn anodes demonstrate an extended lifespan of 2500 h in symmetrical cells and a high Coulombic efficiency of 99.15%.Furthermore,Zn(OTf)_(2)-based system typically exhibits poor stability at high current densities.Fortunately,the lifespan of symmetrical cells was extended by 40-fold at the high current density.When paired with an Na V_(3)O_(8)·1.5H_(2)O(NVO)cathode,the system achieves 86.5%capacity retention after 3000 cycles at a large specific current density of 10 A g^(-1).These results underscore the efficacy of the curcumin-based protective layer in enhancing the reversibility and stability of metal electrodes,specifically relieving the instability of Zn(OTf)_(2)-based systems at high current densities,advancing its commercial viability.
基金supported by the Joint Foundation of National Natural Science Foundation of China and China Academy of Engineering Physics (Grant No 10476007)the Program for New Century Excellent Talents in University (Grant No NCET-05-0799)the Program for Excellent Talents of University of Electronic Science and Technology (Grant No 23601008)
文摘The thermodynamic properties of the ε phase of solid oxygen are studied by using the analytic mean field approach （AMFP）. Analytic expressions for the Helmholtz free energy, internal energy and equation of state of solid oxygen have been derived based on the multi-exponential potential. The formulism for the case of double-exponential （DE） model is applied to the ε phase of solid oxygen. Its four potential parameters are determined through fitting the experimental compression data of the ε phase of solid oxygen. Numerical results of the pressure dependence of the volume calculated by using the AMFP are in good agreement with the original experimental data. This suggests that the AMFP is a useful approach to study the thermodynamic properties of the ε phase of solid oxygen. Furthermore, we predict the variation of the volume, lattice parameters and intermolecular distances with pressure, and some thermodynamic quantities versus volume, at several higher temperatures.
基金supported by the National Natural Science Foundation of China (Grant Nos. 11075035 and 11222544)the Fok Ying Tung Education Foundation,China(Grant No. 131008)+2 种基金the Program for New Century Excellent Talents in University,China (Grant No. NCET-12-0121)the Shanghai Rising-Star Program,China(Grant No. 12QA1400200)the Fundamental Research Funds for the Central Universities,China
文摘It is important to know whether the laws or phenomena in statistical physics for natural systems with non-adaptive agents still hold for social human systems with adaptive agents, because this implies whether it is possible to study or understand social human systems by using statistical physics originating from natural systems. For this purpose, we review the role of human adaptability in four kinds of specific human behaviors, namely, normal behavior, herd behavior, contrarian behavior, and hedge behavior. The approach is based on controlled experiments in the framework of market-directed resource-allocation games. The role of the controlled experiments could be at least two-fold： adopting the real human decision-making process so that the system under consideration could reflect the performance of genuine human beings; making it possible to obtain macroscopic physical properties of a human system by tuning a particular factor of the system, thus directly revealing cause and effect. As a result, both computer simulations and theoretical analyses help to show a few counterparts of some laws or phenomena in statistical physics for social human systems： two-phase phenomena or phase transitions, entropy-related phenomena, and a non-equilibrium steady state. This review highlights the role of human adaptability in these counterparts, and makes it possible to study or understand some particular social human systems by means of statistical physics coming from natural systems.
文摘Since the first demonstrations of nuclear magnetic resonance (NMR) in condensed matter in 1946, the field of NMR has yielded a continuous flow of conceptual advances and methodological innovations that continues today. Much progress has been made in the utilization of solid-state NMR to illuminate molecular structure and dynamics in systems not controllable by any other way. NMR deals with time-dependent perturbations of nuclear spin systems and solving the time-dependent Schrodinger equation is a central problem in quantum physics in general and solid-state NMR in particular. This theoretical perspective outlines the methods used to treat theoretical problems in solid-state NMR as well as the recent theoretical development of spin dynamics in NMR and physics. The purpose of this review is to unravel the versatility of theories in solid-state NMR and to present the recent theoretical developments of spin dynamics.
文摘We study theoretically the electron transport properties in achiral carbon nanotubes under the influence of an external electric field E(t) using Boltzmann’s transport equation to derive the current-density. A negative differential conductivity (NDC) is predicted in quasi-static approximation i.e., ωτ 0 is equal to the amplitude of the AC electric field E1. The peak of the NDC intensity occurs at very weaker fields than that of superlattice under the same conditions. The peak intensity decreases and shifts to right with the increase in the amplitude of the ac field. This mechanism suppresses the domain formation and therefore could be used in terahertz frequency generation.
基金funded by the Science and Technology Project of Tianjin(No.24YDTPJC00680)the National Natural Science Foundation of China(No.52406191).
文摘The growth of computing power in data centers(DCs)leads to an increase in energy consumption and noise pollution of air cooling systems.Chip-level cooling with high-efficiency coolant is one of the promising methods to address the cooling challenge for high-power devices in DCs.Hybrid nanofluid(HNF)has the advantages of high thermal conductivity and good rheological properties.This study summarizes the numerical investigations of HNFs in mini/micro heat sinks,including the numerical methods,hydrothermal characteristics,and enhanced heat transfer technologies.The innovations of this paper include:(1)the characteristics,applicable conditions,and scenarios of each theoretical method and numerical method are clarified;(2)the molecular dynamics(MD)simulation can reveal the synergy effect,micro motion,and agglomeration morphology of different nanoparticles.Machine learning(ML)presents a feasiblemethod for parameter prediction,which provides the opportunity for the intelligent regulation of the thermal performance of HNFs;(3)the HNFs flowboiling and the synergy of passive and active technologies may further improve the overall efficiency of liquid cooling systems in DCs.This review provides valuable insights and references for exploring the multi-phase flow and heat transport mechanisms of HNFs,and promoting the practical application of HNFs in chip-level liquid cooling in DCs.
基金supported by the Science,Technology,and Innovation Commission of Shenzhen Municipality(No.GJHZ20220913143204008)the Shccig-Qinling Program(No.SMYJY202300294C)+3 种基金National Natural Science Foundation of China(Nos.22261142666,52372225,52172237,22305191)the Shaanxi Science Fund for Distinguished Young Scholars(No.2022JC-21)the Research Fund of the State Key Laboratory of Solidification Processing(NPU)China(No.2021-QZ-02).
文摘The stability of perovskite solar cells(PSCs)is adversely affected by nonradiative recombination resulting from buried interface defects.Herein,we synthesize a polyionic liquid,poly(p-vinylbenzyl trimethylam-monium hexafluorophosphate)(PTA),and introduce it into the buried interface of PSCs.The quaternary ammonium cation(N(-CH_(3))^(3+))in PTA can fill the vacancies of organic cations within the perovskite structure and reduce shallow energy level defects.Additionally,the hexafluorophosphate(PF6−)in PTA forms a Lewis acid-base interaction with Pb^(2+)in the perovskite layer,effectively passivating deep en-ergy level defects.Furthermore,hydrogen bonding can be established between organic cations and the PF6−anion,preventing the formation of shallow energy level defects.Through this synergistic mecha-nism,the deep and shallow energy level defects are effectively mitigated,resulting in improved device performance.As a result,the resulting treated inverted PSC exhibits an impressive power conversion ef-ficiency(PCE)of 24.72%.Notably,the PTA-treated PSCs exhibit remarkable stability,with 88.5%of the original PCE retained after undergoing heat aging at 85℃ for 1078 h,and 89.1%of the initial PCE main-tained following continuous exposure to light for 1100 h at the maximum power point.Synergistically suppressing multiple defects at the buried interface through the use of polyionic liquids is a promising way to improve the commercial viability of PSCs.
基金financially supported by the Natural Science Foundation of Guangdong Province(No.2024A1515010639)PolyU Postdoc Matching Fund Scheme(No.1-W327),PolyU Grant(No.1-CE0H)+3 种基金Shenzhen Science and Technology Program(No.ZDSYS20220606100406016)Shenzhen Key Laboratory of Photonics and Biophotonics(No.ZDSYS20210623092006020)National Key Laboratory of Green and Long-Life Road Engineering in Extreme Environment(Shenzhen)(No.868-000003010103)National Natural Science Foundation of China(No.52208272)。
文摘Fueled by the increasing imperative for sustainable energy solutions and the burgeoning emphasis on health awareness,self-powered techniques have undergone notable strides in advancement.Triboelectric nanogenerators(TENGs)stand out as a prominent device capitalizing on the principles of triboelectrification and electrostatic induction to generate electricity or electrical signals.In efforts to augment the electrical output performance of TENGs and broaden their range of applications,researchers have endeavored to refine materials,surface morphology,and structural design.Among them,physical morphological modifications play a pivotal role in enhancing the electrical properties of TENGs by increasing the contact surface area,which can be achieved by building micro-/nano-structures on the surface or inside the friction material.In this review,we summarize the common morphologies of TENGs,categorize the morphologies into surface and internal structures,and elucidate their roles in enhancing the electric output performance of devices.Moreover,we systematically classify the methodologies employed for morphological preparation into physical and chemical approaches,thereby furnishing a comprehensive survey of the diverse techniques.Subsequently,typical applications of TENGs with special morphology divided by energy harvesting and self-powered sensors are presented.Finally,an overview of the challenges and future trajectories pertinent to TENGs is conducted.Through this endeavor,the aim of this article is to catalyze the evolution of further strategies for enhancing performance of TENGs.
基金financial support from the National Natural Science Foundation of China(Grant No.61971201)。
文摘High-resolution transmission electron microscopy(HRTEM)promises rapid atomic-scale dynamic structure imaging.Yet,the precision limitations of aberration parameters and the challenge of eliminating aberrations in Cs-corrected transmission electron microscopy constrain resolution.A machine learning algorithm is developed to determine the aberration parameters with higher precision from small,lattice-periodic crystal images.The proposed algorithm is then validated with simulated HRTEM images of graphene and applied to the experimental images of a molybdenum disulfide(MoS_(2))monolayer with 25 variables(14 aberrations)resolved in wide ranges.Using these measured parameters,the phases of the exit-wave functions are reconstructed for each image in a focal series of MoS_(2)monolayers.The images were acquired due to the unexpected movement of the specimen holder.Four-dimensional data extraction reveals time-varying atomic structures and ripple.In particular,the atomic evolution of the sulfur-vacancy point and line defects,as well as the edge structure near the amorphous,is visualized as the resolution has been improved from about 1.75?to 0.9 A.This method can help salvage important transmission electron microscope images and is beneficial for the images obtained from electron microscopes with average stability.
基金financial support from the Hong Kong Polytechnic University(1-YWC6)the Scientific Research Project of Hubei University of Science and Technology,China(BK202018)。
文摘The sodium-ion battery(SIB)cathode material,Na_(4)Fe_(3)(PO_(4))_(2)(P_(2)O_(7))(NFPP),has become a focal material in both academia and industry due to its low cost,long lifespan,and high safety.In the recent three years,substantial efforts have been devoted to promoting the practical applications of NFPP by optimizing its electrochemical performance and disclosing the reaction mechanisms.Various modification strategies and their effect mechanisms have been explored,and the performance evaluation of NFPP has progressively advanced from laboratory-scale coin cells to practical pouch cell configurations.Nevertheless,there remains a lack of systematic reviews comprehensively assessing the developmental status and application readiness of NFPP.This review critically examines NFPP's fundamental structural characteristics and proposes four key development issues.Then,the latest research advances are introduced with explicit differentiation of design strategies and their mechanistic impacts.Notably,we provide a dedicated discussion on NFPP's current pouch cell performance metrics,while highlighting two critical yet underexplored research directions(enhancing air stability and improving tap density)for commercial viability.
基金supported by the Ministry of Education of the Russian Federation(Project No.1023032300071-6-2.3.1).
文摘An experimental investigation of the dynamics of the interface between two low-viscosity fluids with high density contrast oscillating in a fixed vertical slotted channel has been conducted.It has been found that as the amplitude of the liquid column oscillations increases,parametric oscillations of the interface are excited in the form of a standing wave located in the channel plane.In particular,depending on the interfacial tension,the standing waves have a frequency equal to that of liquid piston oscillations(harmonic response),or half of the frequency of oscillations of the liquid column in the channel(subharmonic response).The detected type of instability has a gravitational-capillary nature and is analogous to Faraday waves.The analysis of the overcritical dynamics of wave oscillations indicates that interfacial tension plays a crucial role in determining the type of parametric instability.At high interfacial tension,only synchronous(harmonic)wave modes are observed,and the threshold of the wave excitation is determined by the amplitude of piston oscillations of the liquid column.In this case,the oscillation acceleration does not play a role and has a small value in the threshold of the synchronous mode response.In the case of weak surface tension,subharmonic oscillations are observed.The threshold for the development of these oscillations is determined by the dimensionless acceleration of the oscillating liquid column and remains almost constant with variations in the dimensionless frequency of oscillations.At moderate values of interfacial tension(in the region of moderate dimensionless frequencies),a synchronous wave mode emerges in the stability threshold of the oscillating interface.As the dimensionless acceleration is increased further,a subharmonic mode is excited.The growth of subharmonic oscillations occurs against the background of harmonic wave oscillations,with the oscillations of the interface representing a combination of two standing waves.
基金the European Union,the SOLiD project(grant agreement no.101069505),for the financial support。
文摘LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811)is an attractive material for high-energy-density Li-ion batteries in electric vehicles.However,it suffers from rapid capacity fading.Previous studies have shown that tuning the positive electrode material via atomic layer deposition(ALD)can enhance the electrochemical performance of the material.In this article,we introduce a novel coating method using gaseous precursors in an ALD reactor,where an AlO_(x)layer is deposited directly on the surface of the NMC811 precursor,followed by lithiation.The AlO_(x)coating is applied to the NMC811 powder substrate by exposing it to gas-phase precursors,using a conventional ALD and simplified ALD(chemical vapor deposition-like)method.It is observed that the novel methods lead to the incorporation of Al as a dopant within the bulk of NMC811,rather than forming a conformal AlO_(x)coating,after the final lithiation step.The optimized procedures result in positive electrode materials with higher capacity and enhanced cycling stability in both half-cell and full-cell configurations.Doping or coating was shown to mitigate transition metal dissolution,reduce side reactions between the active material and electrolyte,and improve structural stability.
基金supported by the National Natural Science Foundation of China(Grant Nos.11633001,11920101003,and 12205222 for S.H.)the Key Program of the National Natural Science Foundation of China(Grant No.12433001)+1 种基金the Strate-gic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB23000000)the National Key Research and Development Program of China(Grant No.2021YFC2203001 for Z.C.Z.).
文摘The gravitational memory effect manifests gravitational nonlinearity,degenerate vacua,and asymptotic symmetries;its detection is considered challenging.We propose using a space-borne interferometer to detect memory signals from stellar-mass binary black holes(BBHs),typically targeted by ground-based detectors.We use DECIGO detector as an example.Over 5 years,DECIGO is estimated to detect approximately 2,036 memory signals(SNRs>3)from stellar-mass BBHs.Simulations used frequency-domain memory waveforms for direct SNR estimation.Predictions utilized a GWTC-3 constrained BBH population model(Power law+Peak mass,DEFAULT spin,Madau-Dickinson merger rate).The analysis used conservative lower merger rate limits and considered orbital eccentricity.The high detection rate stems from strong memory signals within DECIGO’s bandwidth and the abundance of stellar-mass BBHs.This substantial and conservative detection count enables statistical use of the memory effect for fundamental physics and astrophysics.DECIGO exemplifies that space interferometers may better detect memory signals from smaller mass binaries than their typical targets.Detectors in lower frequency bands are expected to find strong memory signals from∼10^(4)M⊙binaries.
基金supported by the National Natural Science Foundation of China(Grant No.11574153)the Fund of No.TSXK2022D007。
文摘This paper investigates the influence of filling fraction on the segregation patterns of binary granular mixtures in a vertically vibrating drum through experiments and simulations.Glass and stainless steel spherical grains,which differ in mass density,are used to give rise to density-driven segregation.The results reveal four segregation patterns,including Brazil nut effect segregation,counterclockwise two-eye-like segregation,dumpling-like segregation and clockwise twoeye-like segregation.The theoretical analysis demonstrates that grains predominantly exhibit counterclockwise convection at low filling fractions,while clockwise convection dominates at high filling fractions.Competition between buoyancy and convection forces determines the final stable segregation pattern.These findings provide valuable insights into controlling segregation in granular systems,which is crucial for optimizing industrial processes in fields such as pharmaceuticals and chemical engineering.
基金support from the National Natural Science Foundation of China(No.22308378,22308380,22393963)the Science Foundation of China University of Petroleum,Beijing(No.2462023XKBH005,ZX20230078).
文摘Iron-chromium flow batteries(ICRFBs)have emerged as an ideal large-scale energy storage device with broad application prospects in recent years.Enhancement of the Cr^(3+)/Cr^(2+)redox reaction activity and inhibition of the hydrogen evolution side reaction(HER)are essential for the development of ICRFBs and require a novel catalyst design.However,elucidating the underlying mechanisms for modulating catalyst behaviors remains an unresolved challenge.Here,we show a novel precisely controlled preparation of a novel thermal-treated carbon cloth electrode with a uniform deposit of low-cost indium catalyst particles.The density functional theory analysis reveals the In catalyst has a significant adsorption effect on the reactants and improves the redox reaction activity of Cr^(3+)/Cr^(2+).Moreover,H+is more easily absorbed on the surface of the catalyst with a high migration energy barrier,thereby inhibiting the occurrence of HER.The assembled ICRFBs have an average energy efficiency of 83.91%at 140 mA cm^(-2),and this method minimizes the electrodeposition process and cleans the last obstacle for industry long cycle operation requirements.The ICRFBs exhibit exceptional long-term stability with an energy efficiency decay rate of 0.011%per cycle at 1000 cycles,the lowest ICRFBs reported so far.Therefore,this study provides a promising strategy for developing ICRFBs with low costs and long cycle life.
基金funded by the National Natural Science Foundation of China(No.22379052)Taishan Scholars of Shandong Province,China(No.tsqnz20221143)。
文摘The effects of synthesis conditions,especially the heating rate,on the reaction kinetics of Ni-rich cathodes were systematically studied.The growth rate of Ni-rich oxide increases continuously as the heating rate increases.Ab initio molecular dynamics simulations demonstrate that a high heating rate induces anabatic oscillations,indicating a decrease in thermodynamic stability and a tendency for the crystal surface to undergo reconstruction.The presence of an intermediate phase at the grain boundary amplifies atomic migration-induced interface fusion and consequently augments crystal growth kinetics.However,the excessively high heating rate aggravates the Li+/Ni2+mixing in the Ni-rich cathode.The single-crystal Ni-rich cathode exhibits enhanced structural/thermal stability but a decreased specific capacity and rate performance compared with its polycrystalline counterpart.
